Hydrogels, formed as capsules, have been adapted as carrier devices for holding/delivering various molecules of interest that can be deposited within the core spaces of hydrogels. Typically, due to technical limitations, the molecules of interest were suspended in oil-based solvents resulting in a capsule structure comprising a hydrophobic core enclosed by a hydrophilic hydrogel matrix that can support substantial amounts of water (e.g., at least 70%). Such hydrogels comprising a hydrophobic core can be of limited use for many applications. The development of more advanced hydrogels comprising a hydrophilic core have been challenging because such capsules cannot maintain the phase separation between the hydrophilic core and the hydrophilic-hydrogel shell matrix, resulting in hydrogel capsules that exhibit sub-optimal properties, and therefore, are inadequate for long-term storage and/or prolonged usage.